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CN1753219A - The manufacture method of a kind of fuel cell, its catalyst layer and this catalyst layer - Google Patents

The manufacture method of a kind of fuel cell, its catalyst layer and this catalyst layer Download PDF

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CN1753219A
CN1753219A CNA200410051683XA CN200410051683A CN1753219A CN 1753219 A CN1753219 A CN 1753219A CN A200410051683X A CNA200410051683X A CN A200410051683XA CN 200410051683 A CN200410051683 A CN 200410051683A CN 1753219 A CN1753219 A CN 1753219A
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fuel cell
catalyst layer
tubular
catalyst
carrier
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CN100395909C (en
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黄文正
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Hongfujin Precision Industry Shenzhen Co Ltd
Hon Hai Precision Industry Co Ltd
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Hongfujin Precision Industry Shenzhen Co Ltd
Hon Hai Precision Industry Co Ltd
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    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
    • Y02P70/00—Climate change mitigation technologies in the production process for final industrial or consumer products
    • Y02P70/50—Manufacturing or production processes characterised by the final manufactured product

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Abstract

本发明提供一种燃料电池催化剂层，其包括一管状载体及形成在该管状载体表面上的催化剂。其中，该管状载体包括纳米管状的金属或导电性氧化物，催化剂沉积形成在该纳米管内壁表面及外壁表面。本发明还提供上述燃料电池催化剂层的制造方法以及具有该催化剂层的燃料电池。本发明所提供的燃料电池催化剂层具有纳米管状结构，有助于实现反应气体与催化剂充分接触，从而增加催化剂活性，提高燃料电池效率。

Figure 200410051683

The invention provides a fuel cell catalyst layer, which includes a tubular carrier and a catalyst formed on the surface of the tubular carrier. Wherein, the tubular carrier includes nanotube-shaped metal or conductive oxide, and the catalyst is deposited and formed on the inner wall surface and the outer wall surface of the nanotube. The present invention also provides a method for manufacturing the fuel cell catalyst layer and a fuel cell with the catalyst layer. The catalyst layer of the fuel cell provided by the invention has a nanotube structure, which is helpful to realize sufficient contact between the reaction gas and the catalyst, thereby increasing the activity of the catalyst and improving the efficiency of the fuel cell.

Figure 200410051683

Description

The manufacture method of a kind of fuel cell, its catalyst layer and this catalyst layer
[technical field]
The invention relates to calalyst layer of fuel cell, particularly a kind of manufacture method with fuel cell, its catalyst layer and this catalyst layer of catalyst carrier.
[background technology]
Fuel cell is by a kind of Blast Furnace Top Gas Recovery Turbine Unit (TRT) that electrochemical reaction produces electric energy taking place, for accelerating the speed of electrochemical reaction, all be formed with a catalyst layer on the electrode, and with catalyst cupport on a carrier material.At present, the catalyst carrier of fuel cell adopts the material of high surface mostly, as material with carbon elements such as the carbon black of nano-noble metal powder and tool high surface or graphite are fully mixed, spread upon on the dielectric film after forming jelly, effective dispersing nanometer size noble metal, form the conductive catalyst layer of fuel cell, can improve catalyst performance and reduce cost.
The U.S. the 4th as bulletin on October 1 nineteen eighty-three, 407, No. 906 patent discloses a kind of electrode that contains the Pt/Pd electrocatalyst layers, this electrode comprises graphitization or the graphited carbon carrier of part, the carbon carrier surface is formed with Pt/Pd catalyst and hydrophobic polymer, and Pd content is 20～65wt% in the Pt/Pd catalyst.But although this conductive carbon material carrier has high surface and effective dispersing nanometer noble metal, the phenomenon that still can not avoid carbon granule to be agglomerated into piece in electrode layer takes place, thereby suppresses the activity site of fuel and oxidant arrival catalyst (as Pt).Industry claims this phenomenon to be " Pt is by latent problem " (Hidden Pt Problem), and it will cause the catalyst practical efficiency to descend, thereby influence electrode performance, finally reduce the efficient of fuel cell.
For solving catalyst by latent problem, the U.S. the 6th that on February 4th, 2004 was announced, 695, No. 986 patent provides a kind of eelctro-catalyst, it comprises nano-scale Pt eelctro-catalyst, a carbon black conductive carrier and silicon gel, it to the carbon black support modification, can strengthen the eelctro-catalyst activity by the silicon gel to a certain extent.But the silicon gel is easy to solidify, and with easier sclerosis after carbon black mixes, causes gas communication to be obstructed, and influences the electrode catalyst performance.
In addition, the catalyst carrier of utilizing other material to make electrode is arranged also, the 6th, 117, No. 581 patents of the U.S. of bulletin disclosed a kind of fuel cell electrode that utilizes conductivity zeolites as catalysts carrier material as on September 12nd, 2000.See also Fig. 1 and Fig. 2, anode 20 and negative electrode 22 (as shown in Figure 1) that fuel cell 10 comprises dielectric film 12 and lays respectively at dielectric film 12 both sides.Anode 20 and negative electrode 22 structures are identical, are example with negative electrode 22, and it has double-decker: one is carbon-coating 50, comprises graininess material with carbon element carrier 42 and load catalyst granules 40 thereon; Another layer is a zeolite layer 52, comprises particulate zeolite carrier 44 and load catalyst granules 40 thereon, and carbon-coating 50 is between electrolyte 12 and zeolite layer 52.Wherein have continuous duct between carrier, filled conductive material in the duct is as alkali metal ion or conducting polymer.This electrode catalyst agent carrier material is that material with carbon element is combined with zeolite facies, utilize zeolite to increase the catalyst dispersiveness, but it need the filled conductive material to realize the electric conductivity of electrode, will influence gas communication and diffusion, reduce catalyst and contact, and cause the active decline of eelctro-catalyst with fuel.
In view of this, provide a kind of reaction gas circulation of being convenient to, promote it to contact with catalyst, the calalyst layer of fuel cell that increases catalyst activity is necessary in fact.
[summary of the invention]
For solving in the prior art because the performance deficiency of catalyst carrier material, cause the fuel circulation to block, catalyst contacts not enough with fuel, thereby the problem that causes catalyst activity reduction, the object of the present invention is to provide a kind of reaction gas circulation of being convenient to, promote it to contact, increase the calalyst layer of fuel cell of catalyst activity with catalyst.
Another order of the present invention is to provide the manufacture method of above-mentioned calalyst layer of fuel cell.
The present invention further provides fuel cell with this catalyst layer.
For realizing above-mentioned first purpose, the invention provides a kind of calalyst layer of fuel cell, it comprises a tubular carrier and is formed on catalyst on the tubular carrier that wherein, this tubular carrier material is selected from tubular metal or tubulose electroconductive oxide.
Wherein, described tubular metal comprises metals such as Cu, Au, Ag, Ni, and the tubulose electroconductive oxide comprises TiO 2, V 2O 5, Co 3O 4, ZnO or WO 3Deng; Catalyst is selected from noble metal or its combinations such as Pt, Pd, Ru; The caliber scope of described tubular carrier is good with 20 nanometers～80 nanometers below 100 nanometers, and the pipe range scope is below 1 micron, and is good with 100 nanometers～500 nanometers; Catalyst particle size is 3 nanometers～20 nanometers, and it loads the shared mass percent content of body weight at pipe is 10%～20%.
For realizing above-mentioned second purpose, the invention provides the manufacture method of above-mentioned calalyst layer of fuel cell, may further comprise the steps: at electrode or bath surface deposition tubular metal or tubulose electroconductive oxide, to form tubular carrier; Again this tubular carrier is placed the solution that contains catalyst ion, and catalyst granules is separated out in tubular support surfaces, promptly form catalyst layer.
Wherein, described deposition adopts methods such as chemical vapour deposition (CVD), physical vapour deposition (PVD) or electrochemical deposition.
For realizing above-mentioned the 3rd purpose, the invention provides a kind of fuel cell with this catalyst layer, it comprises an electrolyte; And the electrode that lays respectively at the electrolyte both sides, comprise anode and negative electrode; Wherein, have a catalyst layer on described electrode or the electrolyte, comprise a tubular carrier and be formed at catalyst on this tubular carrier, this tubular carrier material is selected from tubular metal or tubulose electroconductive oxide.
Wherein, described electrolyte is selected from proton exchange membrane, soild oxide, phosphoric acid, alkaline solution etc.;
Compared with prior art, provided by the present inventionly be used for metal or the electroconductive oxide that calalyst layer of fuel cell comprises nano tubular structure, has bigger serface, can be evenly dispersed catalyst particle effectively, help the circulation of fuel and oxidant and contact with catalyst, to reduce catalyst consumption, increase catalyst performance, thereby improve fuel cell efficiency.
[description of drawings]
Below in conjunction with accompanying drawing the present invention is described in further detail.
Fig. 1 is the fuel cell structure schematic diagram that contains electrode catalyst layer of prior art.
Fig. 2 is the local enlarged diagram of II partial structure among Fig. 1.
Fig. 3 is the fuel cell structure schematic diagram that utilizes catalyst layer of the present invention.
Fig. 4 all is local enlarged diagrams of IV partial structure among Fig. 3.
[embodiment]
Seeing also Fig. 3, is the fuel cell structure schematic diagram that utilizes catalyst layer of the present invention.Anode 2 and negative electrode 3 that fuel cell comprises electrolyte 1 and lays respectively at electrolyte 1 both sides.With all be formed with catalyst layer 4 on electrolyte 1 contacted anode 2 and negative electrode 3 surfaces.Wherein catalyst layer 4 comprises tubular carrier (figure do not show) and is formed on catalyst on this tubular carrier.The used electrolyte of fuel cell of the present invention is selected from proton exchange membrane, soild oxide, phosphoric acid or alkaline solution etc., wherein, proton exchange membrane can be selected from perfluorinated sulfonic acid type film, polystyrolsulfon acid type film, polytrifluorostyrene sulfonic acid type film, phenolic resins sulfonic acid type film, hydrocarbon membrane etc., soild oxide comprises zirconia etc., and alkaline solution is selected from NaOH or KOH etc.When electrolyte was solid-state form, as proton exchange membrane or soild oxide, then catalyst layer also can form at electrolyte and the contacted surface of electrode.Present embodiment adopts Proton Exchange Membrane Fuel Cells, and then electrolyte 1 comprises proton exchange membrane.
Fuel 5 (as hydrogen or methyl alcohol) is fed to anode 2 earlier, flows to anode 2 lip-deep catalyst layers 4 again and also reacts thereon, is cracked into hydrogen ion (being proton) and electronics.Hydrogen ion is penetrated on the catalyst layer 4 on negative electrode 3 surfaces by electrolyte 1, and electronics flows by external circuit, can provide electric power to external loading.Simultaneously, oxidant gas 6 (as air or oxygen) is transported in the catalyst layer 4 on negative electrode 3 surfaces, combines with electronics and hydrogen ion then to form water.
Seeing also Fig. 4, is IV partial structure enlarged diagram among Fig. 3, catalyst layer enlarged diagram promptly provided by the present invention.Catalyst layer 4 of the present invention is positioned between electrolyte 1 and the anode 2 (figure does not show), and gas can be conducting to electrolyte 1 (as shown in Figure 3) from anode 2.Catalyst layer 4 comprises tubular carrier 7 and is formed on catalyst 8 on the tubular carrier 7.Wherein, this tubular carrier 7 is nanotube-shaped conductivity material, and extends axially anode 2 surfaces by electrolyte 1 surface.Nanotube-shaped metal can be selected from metals such as Cu, Au, Ag, Ni; Electroconductive oxide can be selected from TiO 2, V 2O 5, Co 3O 4, ZnO or WO 3Deng oxide.The caliber scope of nanotube is good with 20 nanometers～80 nanometers below 100 nanometers, and the pipe range scope is below 1 micron, is good with 100 nanometers～500 nanometers, helps fuel 5 smooth and easy circulation in catalyst layer 4.Catalyst 8 is selected from noble metal or its combinations such as Pt, Pd, Ru, and it loads the shared mass percent content of body weight at pipe is 10%～20%.Catalyst 8 is formed on the hollow tubular outer wall surface and the inner wall surface of tubular carrier 6, thereby can obtain the catalyst 8 of full and uniform dispersion.When fuel 5 along nanotube-shaped carrier 7 catalyst layer 4 of flowing through, catalyst 8 can fully contact with fuel, thus performance greater catalytic agent activity.
The present invention also provides the manufacture method of above-mentioned calalyst layer of fuel cell, may further comprise the steps:
(1) at electrode or bath surface deposition tubular metal or tubulose electroconductive oxide, to form the carrier material.When electrolyte is solid-state, during as solid-oxide or solid polymer electrolyte, nanotube-shaped carrier material can be deposited on electrode surface or bath surface; When electrolyte is liquid, during as alkaline solution or phosphoric acid electrolyte, nanotube-shaped carrier material then is deposited on electrode surface.Wherein, electrode surface is its surface that contacts with electrolyte, and bath surface is its surface that contacts with electrode.Deposition can adopt methods such as chemical vapour deposition (CVD), physical vapour deposition (PVD) or electro-deposition.Metal material comprises metals such as Cu, Au, Ag, Ni, and electroconductive oxide comprises TiO 2, V 2O 5, Co 3O 4, ZnO or WO 3Deng.
(2) tubular carrier is placed the solution that contains catalyst ion, as chloroplatinic acid (H 2PtCl 66H 2O) solution is 7～9 o'clock at pH value, and constantly stirring state adds a certain amount of reducing agent (as methyl alcohol) down, and making catalyst is that the Pt atom is separated out, and is deposited on tubular support surfaces, promptly forms catalyst layer.
Wherein, the solution that contains catalyst ion also can adopt the corresponding metal salting liquid, is dissolved in then or is suspended in the alcoholic solutions such as methyl alcohol or ethylene glycol, make metal ion and polyalcohol generation reduction reaction, form nano-sized metal particles, it is deposited on tubular support surfaces, promptly forms catalyst layer.When reduction reaction takes place when, can add the predetermined metal salting liquid, can obtain the alloy type catalyst, as in platinum acid chloride solution, adding nitric acid ruthenium or palladium nitrate, can obtain to load on Pt/Ru or Pt/Pb type catalyst layer on the tubular carrier at last.
According to above-mentioned manufacture method, the caliber of nanotube-shaped metal of gained or electroconductive oxide is good with 20～80 nanometers below 100 nanometers, and the pipe range scope is good below 1 micron with 100～500 nanometers; The gained catalyst particle size is 3～20 nanometers, and it is 10%～20% at the shared mass percent of tubular carrier.

Claims (12)

1.一种燃料电池催化剂层，其包括一载体及形成在该载体表面上的催化剂；其特征在于：该载体为管状载体，包括管状金属或管状导电性氧化物。1. A fuel cell catalyst layer, which includes a carrier and a catalyst formed on the surface of the carrier; it is characterized in that: the carrier is a tubular carrier, including tubular metal or tubular conductive oxide. 2.如权利要求1所述的燃料电池催化剂层，其特征在于所述金属材质选自Cu、Au、Ag、Ni等金属。2. The fuel cell catalyst layer according to claim 1, wherein the metal material is selected from metals such as Cu, Au, Ag, and Ni. 3.如权利要求1所述的燃料电池催化剂层，其特征在于所述管状导电性氧化物选自TiO2、V2O5、Co3O4、ZnO或WO3等。3. The fuel cell catalyst layer according to claim 1, wherein the tubular conductive oxide is selected from TiO 2 , V 2 O 5 , Co 3 O 4 , ZnO or WO 3 . 4.如权利要求2或3所述的燃料电池催化剂层，其特征在于所述管状载体管径在100纳米以下，管长在1微米以下。4. The fuel cell catalyst layer according to claim 2 or 3, characterized in that the diameter of the tubular carrier is less than 100 nanometers, and the length of the tube is less than 1 micron. 5.如权利要求4所述的燃料电池催化剂层，其特征在于所述管状载体管径为20纳米～80纳米，管长为100纳米～500纳米。5 . The fuel cell catalyst layer according to claim 4 , characterized in that the tube diameter of the tubular support is 20 nm to 80 nm, and the tube length is 100 nm to 500 nm. 6.如权利要求1所述的燃料电池催化剂层，其特征在于所述催化剂选自Pt、Pd、Ru贵金属或其组合。6. The fuel cell catalyst layer according to claim 1, characterized in that the catalyst is selected from Pt, Pd, Ru noble metals or combinations thereof. 7.如权利要求6所述的燃料电池催化剂层，其特征在于所述催化剂粒径为3纳米～20纳米。7. The fuel cell catalyst layer according to claim 6, characterized in that the particle size of the catalyst is 3 nm to 20 nm. 8.如权利要求7所述的燃料电池催化剂层，其特征在于所述催化剂在管状载体中所占质量百分数为10％～20％。8. The fuel cell catalyst layer according to claim 7, characterized in that the mass percentage of the catalyst in the tubular carrier is 10%-20%. 9.一种燃料电池催化剂层的制造方法，其包括以下步骤：在电极或电解质表面沉积管状金属或管状导电性氧化物，以形成管状载体；再将该管状载体置于含催化剂离子的溶液中，并使催化剂颗粒在管状载体表面析出，即形成催化剂层。9. A method for manufacturing a fuel cell catalyst layer, comprising the steps of: depositing a tubular metal or a tubular conductive oxide on the surface of an electrode or an electrolyte to form a tubular carrier; then placing the tubular carrier in a solution containing catalyst ions , and the catalyst particles are precipitated on the surface of the tubular carrier, that is, the catalyst layer is formed. 10.如权利要求9所述的燃料电池催化剂层的制造方法，其特征在于所述沉积采用化学气相沉积、物理气相沉积或电沉积等方法。10. The manufacturing method of the fuel cell catalyst layer according to claim 9, characterized in that said deposition adopts methods such as chemical vapor deposition, physical vapor deposition or electrodeposition. 11.一种燃料电池，其包括一电解质，以及分别位于电解质两侧的电极，包括阳极及阴极，所述电极或电解质上具有一催化剂层；其特征在于：该催化剂层包括一管状载体及形成在该管状载体上的催化剂，该管状载体材质选自管状金属或管状导电性氧化物。11. A fuel cell comprising an electrolyte, and electrodes respectively positioned on both sides of the electrolyte, including an anode and a cathode, and a catalyst layer is provided on the electrode or the electrolyte; it is characterized in that: the catalyst layer comprises a tubular carrier and forms For the catalyst on the tubular support, the material of the tubular support is selected from tubular metal or tubular conductive oxide. 12.如权利要求11所述的燃料电池，其特征在于所述电解质选自质子交换膜、固体氧化物、磷酸、碱性溶液。12. The fuel cell according to claim 11, characterized in that the electrolyte is selected from the group consisting of proton exchange membranes, solid oxides, phosphoric acid, and alkaline solutions.
CNB200410051683XA 2004-09-24 2004-09-24 A kind of fuel cell, its catalyst layer and the manufacturing method of this catalyst layer Expired - Fee Related CN100395909C (en)

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Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN102468507A (en) * 2010-11-15 2012-05-23 通用汽车环球科技运作有限责任公司 Fuel cell durability through oxide supported precious metals in membrane
CN102698745A (en) * 2012-06-06 2012-10-03 厦门大学 Titanium dioxide nanotube carried palladium nano catalyst and preparation method of same
CN101439283B (en) * 2007-09-27 2012-12-05 通用汽车环球科技运作公司 Nanotube assembly, bipolar plate and process of making the same
CN102916198A (en) * 2011-08-05 2013-02-06 清华大学 Fuel cell membrane electrode
CN103825003A (en) * 2014-02-27 2014-05-28 浙江大学 A kind of three-dimensional porous Co3O4/Pt/Ni composite electrode and its preparation method and application

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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
US4407906A (en) * 1981-11-03 1983-10-04 Paul Stonehart Fuel cell with Pt/Pd electrocatalyst electrode
US6117581A (en) * 1999-03-15 2000-09-12 Ford Global Technologies, Inc. Fuel cell electrode comprising conductive zeolite support material
EP2223895A1 (en) * 2001-10-30 2010-09-01 JGC Catalysts and Chemicals Ltd. Tubular titanium oxide particles and use of the same
CN1226086C (en) * 2001-12-11 2005-11-09 中国科学院大连化学物理研究所 Solid supported noble metal catalyst and its preparing method
US6695986B1 (en) * 2002-09-25 2004-02-24 The United States Of America As Represented By The Secretary Of The Navy Electrocatalytic enhancement with catalyst-modified carbon-silica composite aerogels

Cited By (9)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN101439283B (en) * 2007-09-27 2012-12-05 通用汽车环球科技运作公司 Nanotube assembly, bipolar plate and process of making the same
US9011667B2 (en) 2007-09-27 2015-04-21 GM Global Technology Operations LLC Nanotube assembly, bipolar plate and process of making the same
CN102468507A (en) * 2010-11-15 2012-05-23 通用汽车环球科技运作有限责任公司 Fuel cell durability through oxide supported precious metals in membrane
CN102916198A (en) * 2011-08-05 2013-02-06 清华大学 Fuel cell membrane electrode
CN102916198B (en) * 2011-08-05 2015-03-11 清华大学 fuel cell membrane electrode
CN102698745A (en) * 2012-06-06 2012-10-03 厦门大学 Titanium dioxide nanotube carried palladium nano catalyst and preparation method of same
CN102698745B (en) * 2012-06-06 2014-01-29 厦门大学 Titanium dioxide nanotube-supported palladium nanocatalyst and preparation method thereof
CN103825003A (en) * 2014-02-27 2014-05-28 浙江大学 A kind of three-dimensional porous Co3O4/Pt/Ni composite electrode and its preparation method and application
CN103825003B (en) * 2014-02-27 2015-11-11 浙江大学 A kind of three-dimensional porous Co 3o 4/ Pt/Ni combination electrode and its preparation method and application

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